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<p>Electrocatalysts alter their structure and composition during reaction, which can in turn create new active/selective phases. Identifying these changes is crucial for determining how morphology controls catalytic properties but the mechanisms by which operating conditions shape the catalyst’s working state are not yet fully understood. In this study, we show using correlated operando microscopy and spectroscopy that as well-defined Cu<sub>2</sub>O cubes evolve under electrochemical nitrate reduction reaction conditions, distinct catalyst motifs are formed depending on the applied potential and the chemical environment. By further matching the timescales of morphological changes observed via electrochemical liquid cell transmission electron microscopy with time-resolved chemical state information obtained from operando transmission soft X-ray microscopy, hard X-ray absorption spectroscopy and Raman spectroscopy, we reveal that Cu<sub>2</sub>O can be kinetically stabilized alongside metallic copper for extended durations under moderately reductive conditions due to surface hydroxide formation. Finally, we rationalize how the interaction between the electrolyte and the catalyst influences the ammonia selectivity.</p>

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Revealing catalyst restructuring and composition during nitrate electroreduction through correlated operando microscopy and spectroscopy

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月24日

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  • Aram Yoon,
  • Lichen Bai,
  • Fengli Yang,
  • Federico Franco,
  • Chao Zhan,
  • Martina Rüscher,
  • Janis Timoshenko,
  • Christoph Pratsch,
  • Stephan Werner,
  • Hyo Sang Jeon,
  • Mariana Cecilio de Oliveira Monteiro,
  • See Wee Chee,
  • Beatriz Roldan Cuenya

摘要

Electrocatalysts alter their structure and composition during reaction, which can in turn create new active/selective phases. Identifying these changes is crucial for determining how morphology controls catalytic properties but the mechanisms by which operating conditions shape the catalyst’s working state are not yet fully understood. In this study, we show using correlated operando microscopy and spectroscopy that as well-defined Cu2O cubes evolve under electrochemical nitrate reduction reaction conditions, distinct catalyst motifs are formed depending on the applied potential and the chemical environment. By further matching the timescales of morphological changes observed via electrochemical liquid cell transmission electron microscopy with time-resolved chemical state information obtained from operando transmission soft X-ray microscopy, hard X-ray absorption spectroscopy and Raman spectroscopy, we reveal that Cu2O can be kinetically stabilized alongside metallic copper for extended durations under moderately reductive conditions due to surface hydroxide formation. Finally, we rationalize how the interaction between the electrolyte and the catalyst influences the ammonia selectivity.